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Ralf Kruger was born in Bonn and studied chemistry, first in Bonn and later in Marburg, where he began to focus on analytical chemistry

Ion formation in MALDI: the cluster ionization mechanism.

CHEMICAL REVIEWS, no. 2 (2003): 427-439

Cited by: 284|Views15
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Abstract

Michael Karas was born in 1952 in Wesel, Germany. In 1982, he received his Ph.D. in physical chemistry after his studies of chemistry at the University of Bonn. In 1983, he joined the research group of Franz Hillenkamp, Department of Physics, University of Frankfurt. In Frankfurt and starting from 1987 in the Institute of Medical Physics/...More

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Introduction
  • Michael Karas was born in 1952 in Wesel, Germany. In 1982, he received his Ph.D. in physical chemistry after his studies of chemistry at the University of Bonn.
Highlights
  • Michael Karas was born in 1952 in Wesel, Germany
  • Ralf Kruger was born in Bonn (Germany) and studied chemistry, first in Bonn and later in Marburg, where he began to focus on analytical chemistry
  • Michael Karas at the University of Frankfurt to work in the field of bioanalytical mass spectrometry
  • While he spent some time on nanoESI-MS and MALDI applications, soon the fundamentals of MALDI, and in particular the elucidation of the state of the analyte in the host matrix crystal, became his major objective. He is about to finish his Ph.D. thesis on that topic and is on the move to join the group of Prof
  • The efficiency of ionization by charge separation is determined by the acid-base properties of both analyte, matrix and additives, and their solvation and incorporation behavior; the starting condition is the analyte in its pH-related form in a cluster and not a neutral analyte molecule in the gas phase which is ionized by proton transfer or abstraction with reactive matrix species
  • In the early days of MALDI, initial experiments with oligonucleotides did not show the complete salts as to be expected by the cluster model, but partial proton neutralization of phosphate groups resulting in a distribution of molecule ion species containing different numbers of sodium and potassium.[112]
Results
  • The efficiency of ionization by charge separation is determined by the acid-base properties of both analyte, matrix and additives, and their solvation and incorporation behavior; the starting condition is the analyte in its pH-related form in a cluster and not a neutral analyte molecule in the gas phase which is ionized by proton transfer or abstraction with reactive matrix species.
  • For the case that A- is the typical deprotonated carboxylic acid, either added or matrix, charge separation into the neutral analyte and anion may be energetically favored; the anionadduct intermediates that are detectable under optimized electrospray conditions are not observed, indicating a too high level of excitation in the MALDI ion generation process.
  • It has been reported that the matrix 3-HPA is advantageous for oligonucleotide analysis especially in the positive ion mode.[123] Besides the already mentioned softness oft this matrix, represented by its high initial velocity, a second feature of this matrix can be important: 3-HPA exists at least partially in the protonated form and can work as counterion for the phosphate group and subsequently lead to enhanced anion neutralization.
  • In the early days of MALDI, initial experiments with oligonucleotides did not show the complete salts as to be expected by the cluster model, but partial proton neutralization of phosphate groups resulting in a distribution of molecule ion species containing different numbers of sodium and potassium.[112] It was found by investigations of modified oligonucleotides, that 3-HPA interacts with the phosphodiester backbone,[124,125,126] which further substantiates the above picture.
  • Since this plume contains electrons, hydrogen atoms[51] and all those matrix ionic species showing up the mass spectra in high abundance, electron- or proton-transfer charge reduction and neutralization, which will become more effective for higher charge states, have been considered.[69] Electron neutralization was experimentally proven to occur for a diquaternary nitrogen compound and for a polynuclear metal complex.[127] it cannot be determined to which extent electron capture or electron transfer, respectively, is responsible for charge reduction in MALDI of biopolymers, since other charge reduction mechanisms lead to the same products.
Conclusion
  • Larger oligomers, which need the matrix cluster emission process to survive the transfer into the gas phase, trap and include contaminant salt into the matrix crystals in order to find their way of charged-cluster ionization; again this is connected to the high initial ion velocity as observed for a typical MALDI process.
Tables
  • Table1: Initial Ion Velocities (v0) of Some Analyte Ions Using Different Matrices analyte
Download tables as Excel
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